
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 Ababhali: 
 
 
 
 
 
 
 
 
 
 
 
 
 
 U-Jaeho Lee U-Tae-Hee Han U-Min-Ho Park U-Dae Yool Jung U-Jeongmin Seo U-Hong-Kyu Seo U-Hyunsu Cho U-Eunhye Kim U-Jin Chung U-Sung-Yool Choi U-Taek-Soo Kim U-Tae-Woo Lee U-Seunghyup Yoo Isishwankathelo I-Graphene-based organic light-emitting diodes (OLEDs) kutshanje ivele njengecandelo elibalulekileyo elibalulekileyo kwizikrini ezizizo zelizwe kunye nezibane, ngokuyintloko ngenxa yesithembiso sabo semithombo yokukhanya egobele kakhulu. Nangona kunjalo, ukusebenza kwazo kube, ngokungcono, kufana nezo zemveliso, ezenziwe nge-indium tin oxide. Sicebisa apha isakhiwo esifanelekileyo sediode esekwe kumnxibelelwano olungaphakathi lwe-TiO2® enembonakalo ephezulu® kunye neendlalwazi zokujova imvuthuluko ezineembonakalo ezisezantsi ezibandakanya i-graphene electrodes, ekhokelela kwisimo esifanelekileyo apho ukuphuculwa yi-cavity resonance kuphakanyiswa kwaye ilahleko kwi-surface plasmon polariton ihlaziywa. Indlela ecetywayo ikhokelela kwi-OLEDs ezibonisa ukusebenza okuphezulu kakhulu kwe-quantum yangaphandle ye-40.8 kunye ne-62.1% (64.7 kunye ne-103% kunye nelensi yebhola esiqingatha) kwiimveliso ezingatshatanga kunye ne-multi-junction, ngokulandelanayo. I-OLEDs eyenziwe kwiipolima ngezo electrodes ziya guga rhoqo kwi-radius ye-2.3 mm, ngokuyinxenye ngenxa yeendlalwazi ze-TiO2® ezinyamezela i-flexural strain ukuya kuthi ga kwi-4% nge-crack-deflection toughening. Intshayelelo Iinzuzo zefom-factor ezinje ngokugoba kunye nokunwebeka ziye zazise i-organic light-emitting diodes (OLEDs) ingqalelo enkulu ukusetyenziswa kwezixhobo ezivelayo ezifana nezixhobo ezinxibayo, ezijijwayo okanye ezisongwayo ezifuna ukuhamba, ukujijeka kunye/okanye ukwanda , . Ukuzaliseka ngokupheleleyo kweso sithunzi, nangona kunjalo, akubanga lula kwaye kufuna umzamo omkhulu kwezinto ezahlukeneyo ezifana nophuhliso lweetekhnoloji ze-thin-film transistor ezingekho phantsi kweedegri ezantsi kunye/okanye ukufakwa okugobayo . Enye into ebalulekileyo ekufuneka iqwalaselwe kwiikrini ezikwazi ukugoba kakhulu kukufumana ii-electrodes ezingabonakaliyo (TEs) ezinokubuyisela ii-electrodes ze-indium tin oxide (ITO), eziye zihlala zihlupheka ngokugoba okulinganiselweyo kunye neengxaki ezinokubakho zemali ezinxulumene nemfuno ephezulu kunye/okanye ukubonelela okungazinzanga . Ngokolu hlobo, iintlobo ezahlukeneyo ii-electrodes eziguquguqukayo ezingabonakaliyo ezifana ne-metal nanowires, izinto ezisekelwe kwikhabhoni (umzekelo, i-carbon nanotubes okanye i-graphene) kunye ne-metal grids ezidibene nezinye iintlobo ze-TEs zicetywa kwi-OLEDs , , , , , . Phakathi kwazo, i-graphene—ilayila ekubuyeni kwayo enomlinganiselo omnye we-sp2-hybridized carbon atoms—iye yagqaliswa njengento ethembisayo kuba ukudibanisa kwayo okwahlukileyo kobukhulu bayo kunye neempawu zombane eziphezulu kulindeleke ukuba kuvumele ii-electrodes ezikhazimulayo ezine-haze okanye ingekho ye-optical, i-surface topology egudileyo kuthintela ukutyhola okubangelwa kukugqabhuka kunye nokonakala, ukuhanjiswa okuphezulu, ukumelana kwe-sheet ephezulu kunye nezinga eliphezulu lokugoba konke ngaxeshanye , . Ukulungiswa ngokulula kwe-graphene ekumgangatho ophezulu kwiikholoni ezinkulu zeplastiki kutshanje kuye kwaboniswa kwi-electrodes ezingabonakaliyo ezineendlela ezihambelana nokuveliswa kobuninzi zii-sectors zezoshishino, zibonisa ukusebenza kwazo okusebenzayo , . Zombini i-single-layer graphene (SLG) kunye ne-multi-layer graphene (MLG) ziye zaboniswa ukuba zine-performance efanelekileyo ye-TEs kwi-OLEDs , . Ngokukodwa, i-OLEDs ezisebenza nge-graphene ziye zafunyanwa ngoncedo lweendlalwazi zokujova imvuthuluko (HILs) ezisetyenziselwa ukoyisa ukumelana kwazo okungaphantsi, okwaziwayo ukuba malunga ne-4.5 eV. Ezi ndlalwazi zokujova zibandakanya ii-polymers ezikhuthazayo ezineempawu zombane ezihambayo ezibizwa ngokuba yi-self-organized gradient HIL (GraHIL) , kunye neendlalwazi ezincinci ze-buffer ze-MoO3® ezidibene nee-polymers ezikhuthazayo ze-poly(3,4-ethylenedioxythiophene): polystyrene sulfonate (PEDOT:PSS) . Nangona kunjalo, ukusebenza kwamandla kunye nokusebenza okuphezulu kwe-quantum yangaphandle (EQE) kwezi-OLEDs ze-graphene ze-state-of-the-art zaziseyimlinganiselo nezo ze-OLEDs ezisekelwe kwi-ITO, ngaphandle kokuba kusetyenziswa ilensi enkulu ye-hemispherical ukuze kuphuculwe ukukhutshwa kwangaphandle . Ukugcina ukusebenza okuphezulu kangangoko kunokwenzeka kubaluleke kakhulu kwiikrini eziguquguqukayo ezisetyenziswa kwizicelo eziphathwayo kakhulu okanye ezinxibayo, kuba zihlala zixhomekeke kwiibhetri ezinomthamo omncinci wamandla ngenxa yezithintelo kubungakanani, ubunzima okanye iifom zeefom. Oku kufuna ukuphuhliswa kwesakhiwo sesixhobo esinokwandisa ukusebenza kwe-OLEDs ezisekelwe kwi-graphene. Umngeni omkhulu kukuphuhlisa isakhiwo okanye indlela yokukhupha ubungakanani bayo obupheleleyo bokubonakala ngelixa kugcinwa izibonelelo ze-graphene kwiifom zeefom kangangoko kunokwenzeka. 1 2 3 4 4 5 6 7 8 9 10 11 11 12 13 14 13 14 14 Ngokolu hlobo, sikhangela isakhiwo sediode esilula esekwe kwiindlalwazi ze-TiO2® enembonakalo ephezulu kunye ne-HILs ezineembonakalo ezisezantsi ezibandakanya ii-electrodes ze-graphene. Ngoyilo olubonakalayo oluthatha inzuzo epheleleyo kumsebenzi ongaphakathi phakathi kweendlalwazi eziphezulu nezingezantsi ezilawula zombini ukuphuculwa kwe-cavity resonance kunye nokulahleka kwi-surface plasmon polariton (SPP), ii-OLEDs ezisekelwe kwi-graphene ezicetywayo zibonisa i-EQE ephezulu engazange ibonwe kwiimveliso ezisebenzisa i-graphene njenge-electrode engabonakaliyo. Ngapha koko, ukumelana okuphezulu okungaqhelekanga kwe-TiO2® kwi-flexural strain kuboniswa okuvumela ii-OLEDs zeplastiki ezingekho nje ezisebenzayo kodwa nazo ziyakwazi ukugoba kakhulu. Iziphumo Uyilo olubonakalayo lwee-OLEDs ezisebenza kakhulu ezisekelwe kwi-graphene Ukusebenza kwe-OLEDs kukhawulwe ngokupheleleyo kukuphuma kwesekeli okungapheliyo okuhlala kujikeleze i-20% ngokungcono kwiimveliso ezinama-emitters angayiyonye i-isotropic. Phakathi kwezibonelelo ezahlukeneyo zokwandisa ukukhutshwa okucetywayo ukuza kuthi ga ngoku , indlela esekwe kwi-microcavity resonance inezibonelelo ekugcineni kwayo ifom ye-planar ngaphandle kokusebenzisa nayiphi na i-micro/nano structuring okanye isakhiwo selensi ukuze ii-OLEDs ezenziwe ngayo zingavezwa zii-short zombane kunye ne-optical artefacts ezingafanelekanga kwisicelo sokubonisa (umzekelo, ukufiphaza, ukukhutshwa kwe-diffraction, njl.njl.) kodwa zinokubonisa imibala eyimveli, egcweleyo ebomvu (R), eluhlaza (G), eluhlaza okwesibhakabhaka (B) kunye nokusebenza okuphuculweyo , . Ngomphumo omncinci kodwa osengqiqweni we-microcavity, ii-OLEDs ezisekelwe kwi-ITO nazo zinokulungiswa ukuze zisebenze kakhulu, ngaphandle kokubangela nayiphi na i-haze okanye ukufiphaza, ngokulungisa ubude beendlalwazi ze-ITO; kwesi sikimu, i-first-order, i-3 /4 yoyilo lwe-cavity, apho   ibhekisa kubude bobude, ifunyenwe kunye nesiphelo esivuliweyo semod yelwa ibekwe kwi-ITO/substrate interface , . Kwimeko ye-ITO-free, ii-OLEDs ezisekelwe kwi-graphene, nangona kunjalo, ii-electrodes ze-graphene azinakwenziwa zibe nazo ubude obungako ukulawula ubude be-cavity, nto leyo eyenza kube ngumngeni ukuphucula ukusebenza ngomphumo wokubuyela kwakhona . 15 16 17 λ λ 18 19 20 Njengenye indlela, umntu unokubeka ilayila enezintso eziphezulu ( H) ngaphantsi kweendlalwazi ze-graphene njengoko kubonisiwe kwi-<a href="https://www.nature.com/articles/ncomms11791#Fig1">Umfanekiso 1a</a> ngendlela efanayo ne-metal-free, i-dielectric capped thin-metal electrodes , , , . Ngenxa yokuba ukukhanya kungadala i-graphene kancinci nje utshintsho lwemilo ngenxa yokuba ibhunga layo incinci, oyilo lwe-cavity ye-3 /4 lunokufunyanwa ngokulula, umzekelo, kunye nobude obubonakalayo be-organic kunye neendlalwazi zokujova kunye neendlalwazi eziphezulu zentsimbi ezibekwe malunga ne-2 /4 kunye ne- /4, ngokulandelanayo (<a href="https://www.nature.com/articles/ncomms11791#Fig1">Umfanekiso 1b</a>). Ngokukodwa, ilayila ephezulu yentsimbi ene-‘ /4-thick’ ikwasebenza njenge-metal-free, i-dielectric mirror enika ukubuyela okubalulekileyo kwi-bottom electrode assembly ( bot) kulutsha olubhekiswe kwiindlalwazi ze-organic, njengoko kunokuqinisekiswa kumagrafu abonisiweyo ngasezantsi kwe-<a href="https://www.nature.com/articles/ncomms11791#Fig1">Umfanekiso 1c,d</a>. Oku kunika ii-OLEDs ezisekelwe kwi-graphene amathuba okuphucula ukusebenza kwazo ngomphumo wokubuyela kwakhona, ongabikho kungenjalo. Kubonisiwe ukuba  bot kunye nokuphuculwa okuhambelanayo kwe-resonance kunyuka kunye  H (<a href="https://www.nature.com/articles/ncomms11791#MOESM1492">Inombolo eyongezelelweyo yefayile ye-SM 1492</a>; Supplementary Fig. 1). Ukubaluleka okuphezulu kukwanenzuzo ngokuphathelele ukugoba kuba ubude obubonakalayo obujolise kuyo ( H H) bunokufumaneka kunye nobude obuncinci  H, kwaye kuba i-crack ebangela ukugoba ye-film ethile idla ngokubakho kwi-strain yokuqala ephantsi kunye nobude obukhulu    . Ilayila enempawu eziphezulu ezimpumeleleyo kwesi sikimu kufuneka ke ibe ne- H enkulu kangangoko kunokwenzeka. Ngapha koko, kufuneka ibe ngumbonakalo, kwaye ngaphezu kwako konke, ayifanele yonakaliswe yinkqubo ethile yokudluliselwa kwe-graphene. Phakathi kwezinto ezininzi ezinokubakho, ilayila ye-TiO2® e-sputtered iyabonakala kuluhlu olubonakalayo kwaye inezintso eziphezulu ( =2.5). Ngokungafani nezinye iindlalwazi eziphezulu esizizamileyo, ilayila ye-TiO2® ijika ibe nokumelana okunamandla kwe-chemical ngokuchasene neenkqubo zokudluliselwa kwe-graphene ezisebenzisa ulwelo, njenge-acetone okanye i-isopropyl alcohol (IPA), ivumela ukubunjwa kwe-graphene ekumgangatho ophezulu phezu kwayo (<a href="https://www.nature.com/articles/ncomms11791#MOESM1492">Inombolo eyongezelelweyo yefayile ye-SM 1492</a>; Supplementary Fig. 2). n 17 20 21 22 λ λ λ λ R R n n d d d 23 n n   ( ) Isakhiwo sesixhobo esicetywayo se-OLEDs. ( ) Ukusasazeka kwamandla ombane (imigca echaziweyo) ye-OLEDs phantsi kophicotho ukuze uyilo lwazo lwe-cavity yokuqala. Ukusasazeka kwamandla ombane kwi-OLEDs ezisekelwe kwi-graphene ngaphandle kwe-TiO2® kuboniswa kunye nokuthelekisa xa ubukhulu beendlalwazi ze-organic bufana nezo ze-OLEDs kunye ne-TiO2® kodwa ngaphandle kwe-HILs ezineembonakalo ezisezantsi. ( , ) Imilinganiselo yokusebenza okuphezulu kwe-quantum yangaphandle ( EQE) ye-OLEDs ezisekelwe kwi-graphene kunye ne-TiO2® engaphantsi njengomsebenzi wobukhulu be-TiO2® kunye ne-organic layer ( TiO2® kunye  org, ngokulandelanayo). Imigca echaziweyo imele imigca yomphakamo we- EQE ye-10, 20, 30 okanye 40% njengoko kuchaziwe kwigrafu. ( ) Ngaphandle kwe-HIL enembonakalo ephantsi; ( ) kunye ne-GraHIL njenge-HIL enembonakalo ephantsi. Ngasezantsi kwicala ngalinye, ukubuyela kwakhona ( bot) kwi-bottom electrode assembly (TiO2®/graphene/(HIL)) njengento ipheleleyo iboniswa njengomsebenzi we- TiO2® kulutsha olubhekiswe kwiindlalwazi ze-organic. a b c d η d d η c d R d Kubalulekile ukwazi ukuba i-micro-cavity structure yohlobo oluphezulu (umzekelo, i-oda lesibini, i-cavity ye-5 /4) esekwe kwisithunzi esityebileyo esingenakwenzeka. Kulo msebenzi, nangona kunjalo, uyilo lwe-cavity yokuqala lwafunyanwa kuqala kuba lubangela i-Purcell effect enamandla kunye nemilo yombane encinci kunoyilo oluphezulu, ekugqibeleni kukhokelela ekusebenzeni okuphezulu kunye ne-EQE , . Iingxaki zisekhona kuyilo lwe-cavity yokuqala kuba indawo efanelekileyo yendawo yokukhutshwa ivele kwi-antinode yokuqala ukusuka kwi-organic/metal interface, nto leyo eyenza kube nzima ukunciphisa iimod yama-SPP ngokwandisa ibanga le-emitter ukuya kwi-metal , . Indlela enye esetyenziswa ngokubanzi ukunciphisa i-SPP kukubandakanya izakhiwo zangaphakathi ezijijwayo okanye ii-corrugations , kodwa ukunyamezela kwi-short zombane kunokuba yingozi ngezi ndlela. Indlela esiyisebenzisayo apha kukubandakanya ilayila enembonakalo ephantsi, eye yabonisa ukuba inciphisa iimod ze-SPP , . Ngokunethamsanqa, i-GraHIL okanye ilayila yokujova imvuthuluko eyenziwe yodwa eyenziwe yi-PEDOT:PSS kunye ne-tetra-fluoroethylene-perfluoro-3, 6-dioxa-4-methyl-7-octenesulphonic acid copolymer (PFI), eyayicetywe ngaphambili ngababhali kwaye yabonisa ukuba iyasebenza kakhulu ekuphuculeni ukujova imvuthuluko kwi-OLEDs ezisekelwe kwi-graphene , inembonakalo ejikeleze i-1.42 kwi-  ye-550 nm (<a href="https://www.nature.com/articles/ncomms11791#MOESM1492">Inombolo eyongezelelweyo yefayile ye-SM 1492</a>; Supplementary Fig. 3), ephantsi kakhulu kunezo zeendlalwazi eziqhelekileyo ze-organic ( =1.8). Ngomnxibelelwano olungaphakathi kweendlalwazi eziphezulu nezingezantsi ezibandakanya ii-graphene layers, ukuphuculwa komphumo wokubuyela kwakhona kwe-cavity kunye nokunciphisa iimod ze-SPP kunokwenziwa ngaxeshanye ukuze i-EQE iphakanyiswe kakhulu nangaphandle kwezakhiwo zokukhupha. λ 24 25 25 26 27 28 29 13 λ n Ukufakwa kwe-<a href="https://www.nature.com/articles/ncomms11791#Fig2">Imifanekiso 2a,b</a> ibonisa iziphumo zokulinganisa ezibonakalayo ezisekelwe kwintengiso yemveli ye-classical electromagnetic theory efingqwe yi-Furno  .  kuluhlu olupheleleyo lolwazi olubonakalayo, naku-<a href="https://www.nature.com/articles/ncomms11791#Fig2"> </a> ye-550 nm. Ifom yendlela iqwalasela i-Purcell factor, impembelelo yokubeka i-dipole, kunye nokuvuselelwa kwiimod ze-SPP kunye ne-waveguide. Ukubandakanywa ngokupheleleyo kwezi zinto zonke kubonwa kubalulekile ekuhlaziyweni okuchanekileyo kunye noyilo oluchaziweyo njengoko ukulinganisa okungaphezulu okanye okungaphantsi kunokwenzeka xa kusetyenziswa indlela elula engayibandakani enye okanye ngaphezulu kwezi ziphumo (bona <a href="https://www.nature.com/articles/ncomms11791#MOESM1492">Inombolo eyongezelelweyo yefayile ye-SM 1492</a>; Inombolo eyongezelelweyo yefayile ye-SM 1492; <a href="https://www.nature.com/articles/ncomms11791#MOESM1492">Ithebhile 1 eyongezelelweyo</a> kunye <a href="https://www.nature.com/articles/ncomms11791#MOESM1492">Inqaku elongezelelweyo 1</a> ngeziphumo). Iziphumo zibonisa ukuba ukusetyenziswa kwe-GraHIL kusasaza kwakhona izabelo zamandla phakathi kweemodali ezahlukeneyo ukuya kwii-wave vectors ezincinci zangaphakathi ukuze amandla afakwe kwiimod ze-SPP ancitshiswe kwaye iicandelo ezikhutshiweyo ziphakanyiswe ngakumbi (<a href="https://www.nature.com/articles/ncomms11791#MOESM1492">Inombolo eyongezelelweyo yefayile ye-SM 1492</a>; Inombolo eyongezelelweyo yefayile ye-SM 5a). Kungabonwa kwakhona kwi-<a href="https://www.nature.com/articles/ncomms11791#MOESM1492">Ithebhile eyongezelelweyo 2</a> ukuba ukusetyenziswa kwelayila ye-TiO2® ngaphantsi kwe-graphene kunciphisa ngokufanelekileyo inani lamandla afakwe kwiimod ezithwala ngombane kunye nezixhobo ze-substrate ngokunyusa i-resonance. Oku kukhokelela ekunyukeni okubalulekileyo kwisikhundla sokukhupha, nangona ilahleko kumandla evanescent nayo iboniswa ukuba inyuka ngenxa yokutshintshwa kweemod ze-transverse-electric waveguide ukuya kuthi ga kwi-wave vectors ephezulu yangaphakathi (<a href="https://www.nature.com/articles/ncomms11791#MOESM1492">Inombolo eyongezelelweyo yefayile ye-SM 1492</a>; Inombolo eyongezelelweyo yefayile ye-SM 5b). Ukusetyenziswa okudibeneyo kweendlalwazi eziphezulu (H) ze-TiO2® kunye nezingezantsi (L) ze-GraHIL, kukhokelela kwisimo esifanelekileyo apho ukuphakanyiswa kwe-resonance kuphezulu, kodwa ilahleko kwiimod ze-SPP/evanescent ihlaziywa. Ngapha koko, ukusetyenziswa okudibeneyo kudala isimo esifana ne-HL-stacks, esisetyenziswa rhoqo kwi-multilayer thin-film coating , kwaye iphakanyisa ngakumbi i-<em>R</em>bot (<a href="https://www.nature.com/articles/ncomms11791#Fig1">Umfanekiso 1d</a>), ivumela ukuphakanyiswa okongezelelweyo kumphumo we-Fabry–Perot resonance. Into eyenza ubuchwepheshe obucetywayo bube yodwa kwaye buphuculwe xa kuthelekiswa nobuchwepheshe obuqhelekileyo bububona umsebenzi ongaphakathi kwezi ndlalwazi eziphezulu nezingezantsi ezivumela ulawulo olubonakalayo lwemiphumo ye-resonance kunye nokulahleka kwe-SPP ukuze kuphunyezwe ukukhutshwa okukhulu; kunye nokuphakanyiswa okongezelelweyo kwe-resonance nge-HL stacking. Kunye neempawu zabo zombane ezihambelanayo (umzekelo, ukujova imvuthuluko okusebenzayo), zonke ezi zibonelelo zibonakalayo zivumela umntu ukuba avule ngokupheleleyo nangaphakathi ubungakanani obufihliweyo obunokuthi ii-OLEDs ezingezizo ze-metal zenze ngokwenene. Iigragrafu zomphumo ezifunyenweyo kwi-EQE ephezulu engabonakaliyo ( EQE (max)) njengomsebenzi wobukhulu be-organic ( org) kunye ne-TiO2® ( TiO2®) eziboniswe kwi-<a href="https://www.nature.com/articles/ncomms11791#Fig1">Umfanekiso 1c,d</a> zibonisa ukuba  EQE (max) ingaba phezulu njengo-44% kwiimveliso ezineendlalwazi ze-GraHIL kunye ne-TiO2® ngelixa ingakhawulelwanga kwi-38% ngaphandle kwe-GraHIL ok et al 19 λ 30 η d d η

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